Worldwide heavy oil and bitumen deposits amount to 9 trillion barrels of oil distributed in over 280 basins around the world, with Canada home to oil sands deposits of 1.7 trillion barrels. The global development of this resource and the increase in oil production from oil sands has caused environmental concerns over the presence of toxic compounds in nearby ecosystems and acid deposition. The contribution of oil sands exploration to secondary organic aerosol formation, an important component of atmospheric particulate matter that affects air quality and climate, remains poorly understood. Here we use data from airborne measurements over the Canadian oil sands, laboratory experiments and a box-model study to provide a quantitative assessment of the magnitude of secondary organic aerosol production from oil sands emissions. We find that the evaporation and atmospheric oxidation of low-volatility organic vapours from the mined oil sands material is directly responsible for the majority of the observed secondary organic aerosol mass. The resultant production rates of 45-84 tonnes per day make the oil sands one of the largest sources of anthropogenic secondary organic aerosols in North America. Heavy oil and bitumen account for over ten per cent of global oil production today, and this figure continues to grow. Our findings suggest that the production of the more viscous crude oils could be a large source of secondary organic aerosols in many production and refining regions worldwide, and that such production should be considered when assessing the environmental impacts of current and planned bitumen and heavy oil extraction projects globally.

Abstract. Top-down approaches to measure total integrated emissions provide verification of bottom-up, temporally resolved, inventory-based estimations. Aircraft-based measurements of air pollutants from sources in the Canadian oil sands were made in support of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring during a summer intensive field campaign between 13 August and 7 September 2013. The measurements contribute to knowledge needed in support of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring. This paper describes the top-down emission rate retrieval algorithm (TERRA) to determine facility emissions of pollutants, using SO 2 and CH 4 as examples, based on the aircraft measurements. In this algorithm, the flight path around a facility at multiple heights is mapped to a two-dimensional vertical screen surrounding the facility. The total transport of SO 2 and CH 4 through this screen is calculated using aircraft wind measurements, and facility emissions are then calculated based on the divergence theorem with estimations of box-top losses, horizontal and vertical turbulent fluxes, surface deposition, and apparent losses due to air densification and chemical reaction. Example calculations for two separate flights are presented. During an upset condition of SO 2 emissions on one day, these calculations are within 5 % of the industryreported, bottom-up measurements. During a return to normal operating conditions, the SO 2 emissions are within 11 % of industry-reported, bottom-up measurements. CH 4 emissions calculated with the algorithm are relatively constant within the range of uncertainties. Uncertainty of the emission rates is estimated as less than 30 %, which is primarily due to the unknown SO 2 and CH 4 mixing ratios near the surface below the lowest flight level.

Large-scale oil production from oil sands deposits in Alberta, Canada has raised concerns about environmental impacts, such as the magnitude of air pollution emissions. This paper reports compound emission rates (E) for 69-89 nonbiogenic volatile organic compounds (VOCs) for each of four surface mining facilities, determined with a top-down approach using aircraft measurements in the summer of 2013. The aggregate emission rate (aE) of the nonbiogenic VOCs ranged from 50 ± 14 to 70 ± 22 t/d depending on the facility. In comparison, equivalent VOC emission rates reported to the Canadian National Pollutant Release Inventory (NPRI) using accepted estimation methods were lower than the aE values by factors of 2.0 ± 0.6, 3.1 ± 1.1, 4.5 ± 1.5, and 4.1 ± 1.6 for the four facilities, indicating underestimation in the reported VOC emissions. For 11 of the combined 93 VOC species reported by all four facilities, the reported emission rate and E were similar; but for the other 82 species, the reported emission rate was lower than E. The median ratio of E to that reported for all species by a facility ranged from 4.5 to 375 depending on the facility. Moreover, between 9 and 53 VOCs, for which there are existing reporting requirements to the NPRI, were not included in the facility emission reports. The comparisons between the emission reports and measurementbased emission rates indicate that improvements to VOC emission estimation methods would enhance the accuracy and completeness of emission estimates and their applicability to environmental impact assessments of oil sands developments.volatile organic compounds | emissions | emission inventory validation | oil sands | aircraft measurements

A field project that includes surface observations, remote sensing, and forecast models provides a better understanding of fog-induced low visibility and improves the parameterization of fog microphysics.

Measurements of black carbon (BC) with a highsensitivity laser-induced incandescence (HS-LII) instrument and a single particle soot photometer (SP2) were conducted upwind, downwind, and while driving on a highway dominated by gasoline vehicles. The results are used with concurrent CO 2 measurements to derive fuel-based BC emission factors for real-world average fleet and heavy-duty diesel vehicles separately. The derived emission factors from both instruments are compared, and a low SP2 bias (relative to the HS-LII) is found to be caused by a BC mass mode diameter less than 75 nm, that is most prominent with the gasoline fleet but is not present in the heavy-duty diesel vehicle exhaust on the highway. Results from both the LII and the SP2 demonstrate that the BC emission factors from gasoline vehicles are at least a factor of 2 higher than previous North American measurements, and a factor of 9 higher than currently used emission inventories in Canada, derived with the MOBILE 6.2C model. Conversely, the measured BC emission factor for heavy-duty diesel vehicles is in reasonable agreement with previous measurements. The results suggest that greater attention must be paid to black carbon from gasoline engines to obtain a full understanding of the impact of black carbon on air quality and climate and to devise appropriate mitigation strategies.

Abstract. Aircraft-based measurements of methane (CH 4 ) and other air pollutants in the Athabasca Oil Sands Region (AOSR) were made during a summer intensive field campaign between 13 August and 7 September 2013 in support of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring. Chemical signatures were used to identify CH 4 sources from tailings ponds (BTEX VOCs), open pit surface mines (NO y and rBC) and elevated plumes from bitumen upgrading facilities (SO 2 and NO y ). Emission rates of CH 4 were determined for the five primary surface mining facilities in the region using two mass-balance methods. Emission rates from source categories within each facility were estimated when plumes from the sources were spatially separable. Tailings ponds accounted for 45 % of total CH 4 emissions measured from the major surface mining facilities in the region, while emissions from operations in the open pit mines accounted for ∼ 50 %. The average open pit surface mining emission rates ranged from 1.2 to 2.8 t of CH 4 h −1 for different facilities in the AOSR. Amongst the 19 tailings ponds, Mildred Lake Settling Basin, the oldest pond in the region, was found to be responsible for the majority of tailings ponds emissions of CH 4 (> 70 %). The sum of measured emission rates of CH 4 from the five major facilities, 19.2 ± 1.1 t CH 4 h −1 , was similar to a single mass-balance determination of CH 4 from all major sources in the AOSR determined from a single flight downwind of the facilities, 23.7 ± 3.7 t CH 4 h −1 . The measured hourly CH 4 emission rate from all facilities in the AOSR is 48 ± 8 % higher than that extracted for 2013 from the Canadian Greenhouse Gas Reporting Program, a legislated facility-reported emissions inventory, converted to hourly units. The measured emissions correspond to an emissions rate of 0.17 ± 0.01 Tg CH 4 yr −1 if the emissions are assumed as temporally constant, which is an uncertain assumption. The emission rates reported here are relevant for the summer season. In the future, effort should be devoted to measurements in different seasons to further our understanding of the seasonal parameters impacting fugitive emissions of CH 4 and to allow for better estimates of annual emissions and year-to-year variability.

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Abstract. We evaluate four high-resolution model simulations of pollutant emissions, chemical transformation, and downwind transport for the Athabasca oil sands using the Global Environmental Multiscale -Modelling Air-quality and Chemistry (GEM-MACH) model, and compare model results with surface monitoring network and aircraft observations of multiple pollutants, for simulations spanning a time period corresponding to an aircraft measurement campaign in the summer of 2013. We have focussed here on the impact of different representations of the model's aerosol size distribution and plume-rise parameterization on model results.The use of a more finely resolved representation of the aerosol size distribution was found to have a significant impact on model performance, reducing the magnitude of the original surface PM 2.5 negative biases 32 %, from −2.62 to −1.72 µg m −3 .We compared model predictions of SO 2 , NO 2 , and speciated particulate matter concentrations from simulations employing the commonly used Briggs (1984) plume-rise algorithms to redistribute emissions from large stacks, with stack plume observations. As in our companion paper (Gordon et al., 2017), we found that Briggs algorithms based on estimates of atmospheric stability at the stack height resulted in under-predictions of plume rise, with 116 out of 176 test cases falling below the model : observation 1 : 2 line, 59 cases falling within a factor of 2 of the observed plume heights, and an average model plume height of 289 m compared to an average observed plume height of 822 m. We used a highresolution meteorological model to confirm the presence of significant horizontal heterogeneity in the local meteorological conditions driving plume rise. Using these simulated meteorological conditions at the stack locations, we found that a layered buoyancy approach for estimating plume rise in stable to neutral atmospheres, coupled with the assumption of free rise in convectively unstable atmospheres, resulted in much better model performance relative to observations (124 out of 176 cases falling within a factor of 2 of the observed plume height, with 69 of these cases above and 55 of these cases below the 1 : 1 line and within a factor of 2 of observed values). This is in contrast to our companion paper, wherein this layered approach (driven by meteorological observations not co-located with the stacks) showed a relatively modest impact on predicted plume heights. Persistent issues with over-fumigation of plumes in the model were linked to a more rapid decrease in simulated temperature with increasing height than was observed. This in turn may have led to overestimates of near-surface diffusivity, resulting in excessive fumigation.